DRIFT Study on Cerium−Tungsten/Titiania Catalyst for Selective Catalytic Reduction of NOx with NH3

催化作用 氮氧化物 选择性催化还原 路易斯酸 化学 无机化学 反应机理 漫反射红外傅里叶变换 大气温度范围 吸附 光催化 物理化学 有机化学 气象学 物理 燃烧
作者
Changhao Liang,Junhua Li,Maofa Ge
出处
期刊:Environmental Science & Technology [American Chemical Society]
卷期号:44 (24): 9590-9596 被引量:637
标识
DOI:10.1021/es102692b
摘要

CeO2/TiO2 and CeO2−WO3/TiO2 catalysts prepared by impregnation method assisted with ultrasonic energy were investigated on the selective catalytic reduction (SCR) of NOx (NO and NO2) by NH3. The catalytic activity of 10% CeO2/TiO2 (CeTi) was greatly enhanced by the addition of 6% WO3 in the broad temperature range of 200−500 °C, the promotion mechanism was proposed on basis of the results of in situ diffuse reflectance infrared transform spectroscopy (DRIFT). When NH3 was introduced into both catalysts preadsorbed with NO + O2, SCR would not proceed except for the reaction between NO2 and ammonia. For CeO2/TiO2 catalysts, coordinated NH3 linked to Lewis acid sites were the main adsorbed ammonia species. When NO + O2 was introduced, all the ammonia species consumed rapidly, indicating that these species could react with NOx effectively. Two different reaction routes, L-H mechanism at low temperature (<200 °C) and E-R mechanism at high temperatures (>200 °C), were presented for SCR reaction over CeO2/TiO2 catalyst. For CeO2−WO3/TiO2 catalysts, the Lewis acid sites on Ce4+ state could be converted to Brønsted acid sites due to the unsaturated coordination of Cen+ and Wn+ ions. When NO + O2 was introduced, the reaction proceeded more quickly than that on CeO2/TiO2. The reaction route mainly followed E-R mechanism in the temperature range investigated (150−350 °C) over CeO2−WO3/TiO2 catalysts. Tungstation was beneficial for the formation of Ce3+, which would influence the active sites of the catalyst and further change the mechanisms of SCR reaction. In this way, the cooperation of tungstation and the presence of Ce3+ state resulted in the better activity of CeO2−WO3/TiO2 compared to that of CeO2/TiO2.
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